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Nanodiamonds containing nitrogen vacancy (NV-) centers show promise for anumber of emerging applications including targeted in vivo imaging andgenerating nuclear spin hyperpolarization for enhanced NMR spectroscopy andimaging. Here, we develop a detailed understanding of the magnetic resonancebehavior of NV- centers in an ensemble of nanodiamonds with random crystalorientations. Two-dimensional optically detected magnetic resonancespectroscopy reveals the distribution of energy levels, spin populations, andtransition probabilities that give rise to a complex spectrum. We identifyovertone transitions that are inherently insensitive to crystal orientation andgive well-defined transition frequencies that access the entire nanodiamondensemble. These transitions may be harnessed for high-resolution imaging andgeneration of nuclear spin hyperpolarization. The data are well described bynumerical simulations from the zero- to high-field regimes, including theintermediate regime of maximum complexity. We evaluate the prospects ofnanodiamond ensembles specifically for nuclear hyperpolarization and show thatfrequency-swept dynamic nuclear polarization may transfer a large amount of theNV- center's hyperpolarization to nuclear spins by sweeping over a small regionof its spectrum.

Understanding the magnetic resonance spectrum of nitrogen vacancy centers in an ensemble of randomly-oriented nanodiamonds